Molecular Characterization of Water-Soluble Aerosol Particle Extracts by Ultrahigh-Resolution Mass Spectrometry: Observation of Industrial Emissions and an Atmospherically Aged Wildfire Plume at Lake Baikal

Schneider, E.; Czech, H.; Popovicheva, O.; Lütdke, H.; Schnelle-Kreis, J.; Khodzher, T.; Rüger, C.P.; Zimmermann, R.

Авторы: Schneider Eric, Czech Hendryk, Popovicheva Olga, Lütdke Hannes, Schnelle-Kreis Jürgen, Khodzher Tamara, Rüger Christopher P., Zimmermann Ralf
Журнал: ACS EARTH AND SPACE CHEMISTRY
Том: 6
Номер: 4
Год издания: 2022
Первая страница: 1095
Последняя страница: 1107
DOI: 10.1021/acsearthspacechem.2c00017
Аннотация: Air pollution over Lake Baikal originating fromanthropogenic emissions as well as wildfire events and secondaryorganic aerosol (SOA) formation poses a threat to this worldheritage ecosystem. During a ship expedition in 2018, ambientaerosol particles were sampled on filters at different locations ofLake Baikal and extracted to obtain the fraction of water-solubleorganic aerosol (WSOA). Subsequent analysis by Fourier transformion cyclotron resonance (FTICR) mass spectrometry withdirect-infusion electrospray ionization (ESI) in both ionizationmodes provides insights into the molecular composition of polarand high-molecular-weight species in WSOA. Light absorptionspectral dependence determined by absorption Ångstrom exponent(AAE) is correlated to summed compound class abundancies toidentify light-absorbing compounds. Most detected species are heavily oxidized, associated with intense atmospheric aging, andcontain significant amounts of nitrogen or sulfur, with the most abundant compound classes being CHO, CHON, and CHOS.Nitrogen-containing species are more frequently found in positive ESI and correlate well with AAE. Oxygen-to-nitrogen ratios (O/N) larger than 3 indicate organic nitrates, and also less oxidized nitrogen species can be linked to brown carbon (BrC). ESI in bothionization modes provides complementary molecular information with, on the one hand, more sensitive detection of high averagecarbon oxidation state (OSC) and low-volatility oxidized organic aerosol species in negative mode, and on the other hand, lower OSC(OSC < 0) species as well as oligomers and potential biomass burning organic aerosol in positive mode. Additionally, a great overlapof sum formulae was found at all sampling sites along the expedition route, regardless of the potential primary emission sources,indicating strong atmospheric aging and mixing, leading to a similar oxidized organic aerosol (OOA) from different primary sources.
Добавил в систему: Поповичева Ольга Борисовна

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Molecular Characterization of Water-Soluble Aerosol Particle Extracts by Ultrahigh-Resolution Mass Spectrometry: Observation of Industrial Emissions and an Atmospherically Aged Wildfire Plume at Lake Baikalстатья

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